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Effect of Vinylene Carbonate as an Electrolyte Additive on the Electrochemical Properties of Micro-Patterned Lithium Metal Anode

미세 패턴화된 리튬금속 전극의 Vinylene Carbonate 첨가제 도입에 따른 전기화학 특성에 관한 연구

  • Jin, Dahee (Department of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST)) ;
  • Park, Joonam (Department of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST)) ;
  • Dzakpasu, Cyril Bubu (Department of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST)) ;
  • Yoon, Byeolhee (Department of Chemical and Biological Engineering, Hanbat National University) ;
  • Ryou, Myung-Hyun (Department of Chemical and Biological Engineering, Hanbat National University) ;
  • Lee, Yong Min (Department of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST))
  • 진다희 (대구경북과학기술원에너지공학전공) ;
  • 박주남 (대구경북과학기술원에너지공학전공) ;
  • ;
  • 윤별희 (한밭대학교화학생명공학과) ;
  • 유명현 (한밭대학교화학생명공학과) ;
  • 이용민 (대구경북과학기술원에너지공학전공)
  • Received : 2019.05.15
  • Accepted : 2019.05.21
  • Published : 2019.05.31

Abstract

Lithium metal anode with the highest theoretical capacity to replace graphite anodes are being reviewed. However, the dendrite growth during repeated oxidation/reduction reaction on lithium metal surface, which results in poor cycle performance and safety issue has hindered its successful implementation. In our previous work, we solved this problem by using surface modification technique whereby a surface pattern on lithium metal anode is introduced. Although the micro-patterned Lithium metal electrode is beneficial to control Li metal deposition efficiently, it is difficult to control the mossy-like Li granulation at high current density ($>2.0mA\;cm^{-2}$). In this study, we introduce vinylene carbonate (VC) electrolyte additive on micro patterned lithium metal anode to suppress the lithium dendrite growth. Owing to the synergetic effect of micro-patterned lithium metal anode and VC electrolyte additive, lithium dendrite at a high current density is dense. As a result, we confirmed that the cycle performance was further improved about 6 times as compared with the reference electrode.

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Fig. 1. (a) Optic images and (b, c) 3D mapping image of 2 cm × 2 cm stainless-steel stamp by using digital microscope.

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Fig. 2. Potential profiles of Li/Li symmetrical cells during galvanostatic cycling [+0.5 mA cm-2 (30 min) → Rest (10min) → -0.5 mA cm-2 (30 min) → Rest (10min)].

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Fig. 3. SEM images of (a, b, c) Reference, (d, e, f) 5 wt% VC with Micro-Patterned Lithium anode after plating with a current density of 2 mA cm -2.

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Fig. 4. Voltage profiles of Li (Ni0.6Co0.2Mn0.2)O2 electrodes (a) without VC and (b) with VC electrolyte additive during precycling.

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Fig. 5. SEM images of (a, c) Reference and (b, d) 5 wt% VC with Micro-patterned lithium metal electrodes after precycling.

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Fig. 6. C 1s XPS spectra of the micro-patterned lithium metal anodes (a) without and (b) with VC after precycling.

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Fig. 7. Electrochemical performance of NCM622/Li cells employing Micro-patterned Lithium metal electrodes with and without VC electrolyte additive (a) Comparison of the discharge capacities of the cells at different discharge rates from 0.5C (0.792 mA cm-2) to 15C (23.76 mA cm-2) while keeping the charge rate constant at 0.5C (0.792 mA cm-2). (b) Cycling performance measured at a rate of 1C (1.584 mA cm-2) between 3.0 V and 4.3 V (vs. Li/Li+) (c) Columbic efficiencies of unit cells relevant to Fig. 7b.

Table 1. HOMO and LUMO energy levels of ethylene carbonate(EC), ethyl methyl carbonate(EMC) and, vinylene carbonate(VC), and their reduction potentials.

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Acknowledgement

Supported by : Ministry of SMEs and Startups(MSS), Korea Institute of Energy Technology Evaluation and Planning (KETEP)

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